Visualizing the Anomalous Charge Density Wave States in Graphene/NbSe₂ Heterostructures

Metallic layered transition metal dichalcogenides (TMDs) host collective many-body interactions, including the competing superconducting and charge density wave (CDW) states. Graphene is widely employed as a heteroepitaxial substrate for the growth of TMD layers and as an ohmic contact, where the graphene/TMD heterostructure is naturally formed. The presence of graphene can unpredictably influence the CDW order in 2D CDW conductors. This work reports the CDW transitions of 2H-NbSe₂ layers in graphene/NbSe₂ heterostructures. The evolution of Raman spectra demonstrates that the CDW phase transition temperatures (T_CDW) of NbSe₂ are dramatically decreased when capped by graphene. The induced anomalous short-range CDW state is confirmed by scanning tunneling microscopy measurements. The findings propose a new criterion to determine the T_CDW through monitoring the line shape of the A_1g mode. Meanwhile, the 2D band is also discovered as an indicator to observe the CDW transitions. First-principles calculations imply that interfacial electron doping suppresses the CDW states by impeding the lattice distortion of 2H-NbSe₂. The extraordinary random CDW lattice suggests deep insight into the formation mechanism of many collective electronic states and possesses great potential in modulating multifunctional devices.